Visible‐light‐driven conversion of CO₂ into chemical fuels is an intriguing approach to address the energy and environmental challenges. In principle, light harvesting and catalytic reactions can be both optimized by combining the merits of homogeneous and heterogeneous photocatalysts; however, the efficiency of charge transfer between light absorbers and catalytic sites is often too low to limit the overall photocatalytic performance. In this communication, it is reported that the single‐atom Co sites coordinated on the partially oxidized graphene nanosheets can serve as a highly active and durable heterogeneous catalyst for CO₂ conversion, wherein the graphene bridges homogeneous light absorbers with single‐atom catalytic sites for the efficient transfer of photoexcited electrons. As a result, the turnover number for CO production reaches a high value of 678 with an unprecedented turnover frequency of 3.77 min⁻¹, superior to those obtained with the state‐of‐the‐art heterogeneous photocatalysts. This work provides fresh insights into the design of catalytic sites toward photocatalytic CO₂ conversion from the angle of single‐atom catalysis and highlights the role of charge kinetics in bridging the gap between heterogeneous and homogeneous photocatalysts.

中文翻译：

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可见光驱动的高周转二氧化碳减排的异质单原子催化剂：电子转移的作用

可见光驱动的将CO ₂转化为化学燃料是解决能源和环境挑战的一种有趣方法。原则上，可以通过结合均相和非均相光催化剂的优点来优化集光和催化反应。然而，光吸收剂和催化部位之间的电荷转移效率通常太低而不能限制整体的光催化性能。在此通报中，据报道，部分氧化的石墨烯纳米片上配位的单原子Co位点可作为CO ₂的高活性和持久性非均相催化剂转换，其中石墨烯将单原子催化位点连接到均质的光吸收剂上，以有效转移光激发电子。结果，CO生产的周转数达到了678的高值，前所未有的周转频率为3.77 min ^-1，优于使用最新的非均相光催化剂获得的周转频率。这项工作从单原子催化的角度为光催化CO ₂转化催化位点的设计提供了新的见识，并强调了电荷动力学在弥合非均相和均相光催化剂之间的差距中的作用。